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- Frankfurt Institute for Advanced Studies (FIAS) (4)
- Medizin (4)
We report measurements of the deuterium content of molecular hydrogen (H2) obtained from a suite of air samples that were collected during a stratospheric balloon flight between 12 and 33 km at 40º N in October 2002. Strong deuterium enrichments of up to 400 permil versus Vienna Standard Mean Ocean Water (VSMOW) are observed, while the H2 mixing ratio remains virtually constant. Thus, as hydrogen is processed through the H2 reservoir in the stratosphere, deuterium is accumulated in H2 . Using box model calculations we investigated the effects of H2 sources and sinks on the stratospheric enrichments. Results show that considerable isotope enrichments in the production of H2 from CH4 must take place, i.e., deuterium is transferred preferentially to H2 during the CH4 oxidation sequence. This supports recent conclusions from tropospheric H2 isotope measurements which show that H2 produced photochemically from CH4 and non-methane hydrocarbons must be enriched in deuterium to balance the tropospheric hydrogen isotope budget. In the absence of further data on isotope fractionations in the individual reaction steps of the CH4 oxidation sequence, this effect cannot be investigated further at present. Our measurements imply that molecular hydrogen has to be taken into account when the hydrogen isotope budget in the stratosphere is investigated.
Robinson, Alan D. ; Millard, Genevieve A. ; Danis, François ; Guirlet, Marielle ; Harris, Neil R. P. ; Lee, Adrian M. ; McIntyre, J. D. ; Pyle, John A. ; Arvelius, Johan ; Dagnesjo, Saga ; Kirkwood, Sheila ; Nilsson, Hampus ; Toohey, Darin W. ; Deshler, Terry ; Goutail, Florence ; Pommereau, Jean-Pierre ; Elkins, James William ; Moore, Fred L. ; Ray, Eric ; Schmidt, Ulrich ; Engel, Andreas ; Müller, Melanie
Balloon-borne measurements of CFC11 (from the DIRAC in situ gas chromatograph and the DESCARTES grab sampler), ClO and O3 were made during the 1999/2000 Arctic winter as part of the SOLVE-THESEO 2000 campaign, based in Kiruna (Sweden). Here we present the CFC11 data from nine flights and compare them first with data from other instruments which flew during the campaign and then with the vertical distributions calculated by the SLIMCAT 3D CTM. We calculate ozone loss inside the Arctic vortex between late January and early March using the relation between CFC11 and O3 measured on the flights. The peak ozone loss (~1200ppbv) occurs in the 440-470K region in early March in reasonable agreement with other published empirical estimates. There is also a good agreement between ozone losses derived from three balloon tracer data sets used here. The magnitude and vertical distribution of the loss derived from the measurements is in good agreement with the loss calculated from SLIMCAT over Kiruna for the same days.
Turbulent fluxes of carbonyl sulfide (COS) and carbon disulfide (CS2) were measured over a spruce forest in Central Germany using the relaxed eddy accumulation (REA) technique. A REA sampler was developed and validated using simultaneous measurements of CO2 fluxes by REA and by eddy correlation. REA measurements were conducted during six campaigns covering spring, summer, and fall between 1997 and 1999. Both uptake and emission of COS and CS2 by the forest were observed, with deposition occurring mainly during the sunlit period and emission mainly during the dark period. On the average, however, the forest acts as a sink for both gases. The average fluxes for COS and CS2 are -93 ± 11.7 pmol m-2 s-1 and -18 ± 7.6 pmol m-2 s-1, respectively. The fluxes of both gases appear to be correlated to photosynthetically active radiation and to the CO2 and \chem{H_2O} fluxes, supporting the idea that the air-vegetation exchange of both gases is controlled by stomata. An uptake ratio COS/CO2 of 10 ± 1.7 pmol m mol-1 has been derived from the regression line for the correlation between the COS and CO2 fluxes. This uptake ratio, if representative for the global terrestrial net primary production, would correspond to a sink of 2.3 ± 0.5 Tg COS yr-1.
A comprehensive set of stratospheric balloon and aircraft samples was analyzed for the position-dependent isotopic composition of nitrous oxide (N2O). Results for a total of 220 samples from between 1987 and 2003 are presented, nearly tripling the number of mass-spectrometric N2O isotope measurements in the stratosphere published to date. Cryogenic balloon samples were obtained at polar (Kiruna/Sweden, 68° N), mid-latitude (southern France, 44° N) and tropical sites (Hyderabad/India, 18° N). Aircraft samples were collected with a newly-developed whole air sampler on board of the high-altitude aircraft M55 Geophysica during the EUPLEX 2003 campaign. For mixing ratios above 200 nmol mol−1, relative isotope enrichments (δ values) and mixing ratios display a compact relationship, which is nearly independent of latitude and season and which can be explained equally well by Rayleigh fractionation or mixing. However, for mixing ratios below 200 nmol mol−1 this compact relationship gives way to meridional, seasonal and interannual variations. A comparison to a previously published mid-latitude balloon profile even shows large zonal variations, justifying the use of three-dimensional (3-D) models for further data interpretation.
In general, the magnitude of the apparent fractionation constants (i.e., apparent isotope effects) increases continuously with altitude and decreases from the equator to the North Pole. Only the latter observation can be understood qualitatively by the interplay between the time-scales of N2O photochemistry and transport in a Rayleigh fractionation framework. Deviations from Rayleigh fractionation behavior also occur where polar vortex air mixes with nearly N2O-free upper stratospheric/mesospheric air (e.g., during the boreal winters of 2003 and possibly 1992). Aircraft observations in the polar vortex at mixing ratios below 200 nmol mol−1 deviate from isotope variations expected for both Rayleigh fractionation and two-end-member mixing, but could be explained by continuous weak mixing between intravortex and extravortex air (Plumb et al., 2000). However, it appears that none of the simple approaches described here can capture all features of the stratospheric N2O isotope distribution, again justifying the use of 3-D models. Finally, correlations between 18O/16O and average 15N/14N isotope ratios or between the position-dependent 15N/14N isotope ratios show that photo-oxidation makes a large contribution to the total N2O sink in the lower stratosphere (possibly up to 100% for N2O mixing ratios above 300 nmol mol−1). Towards higher altitudes, the temperature dependence of these isotope correlations becomes visible in the stratospheric observations.
Balloon-borne stratospheric BrO measurements: comparison with Envisat/SCIAMACHY BrO limb profiles
(2006)
Dorf, Marcel ; Bösch, Hartmut ; Butz, Andre ; Camy-Peyret, Claude C. ; Chipperfield, Martyn P. ; Engel, Andreas ; Goutail, Florence ; Grunow, Katja ; Hendrick, François ; Hrechanyy, Serhiy ; Naujokat, Barbara ; Pommereau, Jean-Pierre ; Van Roozendael, Michel ; Sioris, Christopher E. ; Stroh, Fred ; Weidner, Frank ; Pfeilsticker, Klaus
For the first time, results of all four existing stratospheric BrO profiling instruments, are presented and compared with reference to the SLIMCAT 3-dimensional chemical transport model (3-D CTM). Model calculations are used to infer a BrO profile validation set, measured by 3 different balloon sensors, for the new Envisat/SCIAMACHY (ENVIronment SATellite/SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) satellite instrument. The balloon observations include (a) balloon-borne in situ resonance fluorescence detection of BrO, (b) balloon-borne solar occultation DOAS measurements (Differential Optical Absorption Spectroscopy) of BrO in the UV, and (c) BrO profiling from the solar occultation SAOZ (Systeme d'Analyse par Observation Zenithale) balloon instrument. Since stratospheric BrO is subject to considerable diurnal variation and none of the measurements are performed close enough in time and space for a direct comparison, all balloon observations are considered with reference to outputs from the 3-D CTM. The referencing is performed by forward and backward air mass trajectory calculations to match the balloon with the satellite observations. The diurnal variation of BrO is considered by 1-D photochemical model calculation along the trajectories. The 1-D photochemical model is initialised with output data of the 3-D model with additional constraints on the vertical transport, the total amount and photochemistry of stratospheric bromine as given by the various balloon observations. Total [Bry]=(20.1±2.8)pptv obtained from DOAS BrO observations at mid-latitudes in 2003, serves as an upper limit of the comparison. Most of the balloon observations agree with the photochemical model predictions within their given error estimates. First retrieval exercises of BrO limb profiling from the SCIAMACHY satellite instrument agree to <±50% with the photochemically-corrected balloon observations, and tend to show less agreement below 20 km.
Engel, Andreas ; Bönisch, Harald ; Brunner, Dominik ; Fischer, Herbert ; Franke, Harald ; Günther, Gebhard ; Gurk, Christian Thomas ; Hegglin, Michaela I. ; Hoor, Peter ; Königstedt, Rainer ; Krebsbach, Michael ; Maser, Rolf ; Parchatka, Uwe ; Peter, Thomas ; Schell, Dieter ; Schiller, Cornelius ; Schmidt, Ulrich ; Spelten, Nicole ; Szabo, T. ; Weers, Uwe ; Wernli, Heini ; Wetter, Thomas ; Wirth, Volkmar
During SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) we performed measurements of a wide range of trace gases with different lifetimes and sink/source characteristics in the northern hemispheric upper troposphere (UT) and lowermost stratosphere (LMS). A large number of in-situ instruments were deployed on board a Learjet 35A, flying at altitudes up to 13.7 km, at times reaching to nearly 380 K potential temperature. Eight measurement campaigns (consisting of a total of 36 flights), distributed over all seasons and typically covering latitudes between 35° N and 75° N in the European longitude sector (10° W–20° E), were performed. Here we present an overview of the project, describing the instrumentation, the encountered meteorological situations during the campaigns and the data set available from SPURT. Measurements were obtained for N2O, CH4, CO, CO2, CFC12, H2, SF6, NO, NOy, O3 and H2O. We illustrate the strength of this new data set by showing mean distributions of the mixing ratios of selected trace gases, using a potential temperature – equivalent latitude coordinate system. The observations reveal that the LMS is most stratospheric in character during spring, with the highest mixing ratios of O3 and NOy and the lowest mixing ratios of N2O and SF6. The lowest mixing ratios of NOy and O3 are observed during autumn, together with the highest mixing ratios of N2O and SF6 indicating a strong tropospheric influence. For H2O, however, the maximum concentrations in the LMS are found during summer, suggesting unique (temperature- and convection-controlled) conditions for this molecule during transport across the tropopause. The SPURT data set is presently the most accurate and complete data set for many trace species in the LMS, and its main value is the simultaneous measurement of a suite of trace gases having different lifetimes and physical-chemical histories. It is thus very well suited for studies of atmospheric transport, for model validation, and for investigations of seasonal changes in the UT/LMS, as demonstrated in accompanying and elsewhere published studies.
Engel, Andreas ; Möbius, Tanja ; Haase, Hans-Peter ; Bönisch, Harald ; Wetter, Thomas ; Schmidt, Ulrich ; Levin, Ingeborg ; Reddmann, Thomas ; Oelhaf, Hermann ; Wetzel, Gerald ; Grunow, Katja ; Huret, Nathalie ; Pirre, Michel
During several balloon flights inside the Arctic polar vortex in early 2003, unusual trace gas distributions were observed, which indicate a strong influence of mesospheric air in the stratosphere. The tuneable diode laser (TDL) instrument SPIRALE (Spectroscopie InFrarouge par Absorption de Lasers Embarqués) measured unusually high CO values (up to 600 ppb) on 27 January at about 30 km altitude. The cryosampler BONBON sampled air masses with very high molecular Hydrogen, extremely low SF6 and enhanced CO values on 6 March at about 25 km altitude. Finally, the MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) Fourier Transform Infra-Red (FTIR) spectrometer showed NOy values which are significantly higher than NOy* (the NOy derived from a correlation between N2O and NOy under undisturbed conditions), on 21 and 22 March in a layer centred at 22 km altitude. Thus, the mesospheric air seems to have been present in a layer descending from about 30 km in late January to 25 km altitude in early March and about 22 km altitude on 20 March. We present corroborating evidence from a model study using the KASIMA (KArlsruhe Simulation model of the Middle Atmosphere) model that also shows a layer of mesospheric air, which descended into the stratosphere in November and early December 2002, before the minor warming which occurred in late December 2002 lead to a descent of upper stratospheric air, cutting of a layer in which mesospheric air is present. This layer then descended inside the vortex over the course of the winter. The same feature is found in trajectory calculations, based on a large number of trajectories started in the vicinity of the observations on 6 March. Based on the difference between the mean age derived from SF6 (which has an irreversible mesospheric loss) and from CO2 (whose mesospheric loss is much smaller and reversible) we estimate that the fraction of mesospheric air in the layer observed on 6 March, must have been somewhere between 35% and 100%.
Siebert, Stefan ; Döll, Petra ; Hoogeveen, Jippe ; Faures, Jean-Marc ; Frenken, Karen ; Feick, Sebastian
A new version of a digital global map of irrigation areas was developed by combining irrigation statistics for 10 825 sub-national statistical units and geo-spatial information on the location and extent of irrigation schemes. The map shows the percentage of each 5 arc minute by 5 arc minute cell that was equipped for irrigation around the year 2000. It is thus an important data set for global studies related to water and land use. This paper describes the data set and the mapping methodology and gives, for the first time, an estimate of the map quality at the scale of countries, world regions and the globe. Two indicators of map quality were developed for this purpose, and the map was compared to irrigated areas as derived from two remote sensing based global land cover inventories.
Flow velocity in rivers has a major impact on residence time of water and thus on high and low water as well as on water quality. For global scale hydrological modeling only very limited information is available for simulating flow velocity. Based on the Manning-Strickler equation, a simple algorithm to model temporally and spatially variable flow velocity was developed with the objective of improving flow routing in the global hydrological model of Water- GAP. An extensive data set of flow velocity measurements in US rivers was used to test and to validate the algorithm before integrating it into WaterGAP. In this test, flow velocity was calculated based on measured discharge and compared to measured velocity. Results show that flow velocity can be modeled satisfactorily at selected river cross sections. It turned out that it is quite sensitive to river roughness, and the results can be optimized by tuning this parameter. After the validation of the approach, the tested flow velocity algorithm has been implemented into the WaterGAP model. A final validation of its effects on the model results is currently performed.
Maiduguri, an important city in the Sudano-Sahelian zone of West Africa, experiences both drought and floods. Although droughts are more popular, floods are a seasonal occurrence in parts of the city in the average rainy season. Both hazards exert a heavy toll on their victims. Present response to the hazard problems is characterised by a fire-fighting approach which does little about future occurrence. Much of the perception and response is spiritual and stops short of needed structural and organisational programmes for effective mitigation of hazards. Future occurrences of drought and flood may have more adverse effects as land use in the city becomes more complex and agricultural and water supply system comes to depend heavily on surfacial sources. Future effects will also depend on the socio-economic conditions of the people at risk and the capacity of those who help them. Governments and people need to work together to reduce drought and flood hazards.